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One-Pot Synthesis of Pd@PtnL Core-Shell Icosahedral Nanocrystals in High Throughput through a Quantitative Analysis of the Reduction Kinetics.
Chemistry : a European Journal 2019 Februrary 16
We report a one-pot method for the facile synthesis of Pd@PtnL (nL denotes the number of Pt atomic layers) core-shell icosahedral nanocrystals. The success of this method relies on the use of Na2PdCl4 and Pt(acac)2 as the precursors to Pd and Pt atoms, respectively. Our quantitative analysis of the reduction kinetics indicates that the Pd(II) and Pt(II) precursors are sequentially reduced with a major gap between the two events. Specifically, the Pd(II) precursor is reduced first, leading to the formation of Pd-based icosahedral seeds with a multiply-twinned structure. In contrast, the Pt(II) precursor prefers to take a surface reduction pathway on the just-formed icosahedral seeds. As such, the otherwise extremely slow reduction of the Pt(II) precursor can be dramatically accelerated through an autocatalytic process for the deposition of Pt atoms as a conformal shell on each Pd icosahedral core. Compared to the conventional approach to seed-mediated growth, the throughput for the one-pot synthesis of Pd@PtnL core-shell nanocrystals can be increased by more than 30 folds. When used as catalysts, the [email protected] core-shell icosahedral nanocrystals show specific and mass activities of 0.83 mA cm-2 and 0.39 A mgPt-1, respectively, toward oxygen reduction. The Pt-based nanocages derived from the core-shell nanocrystals also show enhanced specific (1.45 mA cm-2) and mass activities (0.75 A mgPt-1), which are 3.8 and 3.3 times greater than those of the commercial Pt/C, respectively.
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